4.5 Article

Encapsulating Semiconductor Quantum Dots in Supramolecular Metal-Organic Frameworks for Superior Photocatalytic Hydrogen Evolution

Journal

ADVANCED MATERIALS INTERFACES
Volume 9, Issue 1, Pages -

Publisher

WILEY
DOI: 10.1002/admi.202101678

Keywords

heterostructures; hydrogen generation; photocatalysis; quantum dots; supramolecular metal organic frameworks

Funding

  1. National Natural Science Foundation of China [21872039, 21974027, 22072030]
  2. Science and Technology Commission of Shanghai Municipality [18JC1411700, 19DZ2270100]

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A novel water dispersible supramolecular metal organic framework (SMOF) has been developed as a platform to encapsulate CdS quantum dots for enhanced solar-induced hydrogen production activity. The strong electrostatic interaction and light-induced charge transfer between SMOF and CdS QDs, combined with high surface area and water dispersible nature, contribute to the distinguished photocatalytic performance. This work not only demonstrates the versatile and effective role of water dispersible SMOF in boosting photocatalytic H-2-production performance, but also lays the foundation for the design and synthesis of SMOF-based heterostructures for general catalysis applications.
Solar-to-hydrogen conversion is a sustainable way of producing renewable fuels, yet the efficiency is limited by the poor photo-induced charge-carrier separation on electrode surface. Developing active and stable hydrogen evolution photocatalysts is challenging and entails intelligent material structure design and tailoring. Here, a novel water dispersible supramolecular metal organic framework (SMOF) is employed as a general and high-performance platform to encapsulate CdS quantum dots (QDs) for achieving highly improved solar-induced H-2-production activity. Particularly, the CdS QDs@SMOF heterostructure exhibits an excellent H-2 generation activity of 49.4 mu mol h(-1) (TOF = 47.0/h), exceeding those of most reported heterogeneous metal organic frameworks-based photocatalytic systems. Advanced characterizations disclose that the strong electrostatic interaction and light-induced charge transfer between SMOF and CdS QDs, combined with the high surface area, water dispersible nature, and abundant reactive centers synergistically contribute to this distinguished photocatalytic performance. The work not only demonstrates the water dispersible SMOF can serve as a versatile and effective platform supporting semiconductor to boost the photocatalytic H-2-production performance without co-catalysts, but also paves avenues to the design and synthesis of SMOF-based heterostructures for general catalysis applications.

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